The set consists of 63 CDs, the majority of which are reissues of 59 albums released by Cash during his 1958–1986 tenure with Columbia. Each CD is packaged in a replica of the original LP cover, with any albums originally issued as two-LP set condensed onto one disc with the exception of The Gospel Road which remains in a two-CD configuration. Bonus material includes a two-CD set titled The Singles, Plus, compiling non-album tracks and duets taken from other albums; a Carter Family album on which Cash provided guest vocals; the two albums Cash recorded for Columbia as a member of the supergroup The Highwaymen; and an extended edition of the Sun Records album With His Hot and Blue Guitar with additional tracks from the Sun era (including the complete contents of his second Sun album, Sings the Songs That Made Him Famous). Hot and Blue Guitar is the only album to be presented in an extended edition; all other albums are featured with their original contents, without augmentation. As such this is not a complete survey of everything Cash recorded for Columbia; for example, additional performances from the At Folsom Prison and At San Quentin live shows, included on separate reissues of the two albums, are not included. Also omitted is the 1975 album Destination Victoria Station which had featured new performances of previously released recordings, the 1961 album The Lure of the Grand Canyon, the 1980 gospel album A Believer Sings the Truth, as well as most of the tracks issued on Columbia's Bootleg series of 2011–2012.Out Among the Stars, a complete album recorded by Cash in the early 1980s but not released at that time, is also omitted as it would not be released officially until 2014.
Many of the albums featured in the set make their CD debut in the collection. According to country historian Rich Kienzle's liner notes (part of a 200-page book included in the set), one album Koncert V Praze (In Prague–Live) received its first North American release in the set.
^The four-volume Bootleg series, released under Columbia-Legacy in 2011–2012, consists of four sets of rare and mostly previously unreleased Cash recordings: Vol. 1 features home recordings and demos (which had previously been issued as Personal File in 2006); Vol. 2 features Sun demos, a transcribed episode of the Johnny Cash Show radio program from 1955, rare singles (not all of which are included in The Singles, Plus) and unissued recordings; Vol. 3 compiles live recordings dating from the 1950s to 1979; Vol. 4 compiles Gospel recordings, including the contents of two albums recorded during Cash's Columbia tenure but initially released by other labels, and a complete third album that was never released.
^Rich Kienzle, writing in Johnny Cash: The Complete Columbia Album Collection liner notes, 2012, p. 29